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Title: The key energy scales of Gd-based metallofullerene determined by resonant inelastic x-ray scattering spectroscopy

Endohedral metallofullerenes, formed by encaging Gd inside fullerenes like C 80, can exhibit enhanced proton relaxitivities compared with other Gd-chelates, making them the promising contrast agents for magnetic resonance imaging (MRI). However, the underlying key energy scales of Gd x Sc 3-xN@C 80 (x = 1–3) remain unclear. Here, we carry out resonant inelastic x-ray scattering (RIXS) experiments on Gd xSc 3-xN@C 80 at Gd N 4,5-edges to directly study the electronic structure and spin flip excitations of Gd 4f electrons. Compared with reference Gd 2O 3 and contrast agent Gadodiamide, the features in the RIXS spectra of all metallofullerenes exhibit broader spectral lineshape and noticeable energy shift. Using atomic multiplet calculations, we have estimated the key energy scales such as the inter-site spin exchange field, intra-atomic 4f–4f Coulomb interactions, and spin-orbit coupling. The implications of these parameters to the 4f states of encapsulated Gd atoms are discussed.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ; ORCiD logo [4] ; ORCiD logo [6] ;  [1]
  1. Tamkang Univ., Taipei (Taiwan). Dept. of Physics
  2. New York Univ. (NYU), NY (United States). Dept. of Physics
  3. Lund Univ. (Sweden). MAX IV Lab.
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Univ. of Science and Technology of China, Hefei (China). Hefei National Lab. for Physical Sciences at Microscale, CAS Key Lab. of Materials for Energy Conversion, Dept. of Materials Science and Engineering, Synergetic Innovation Center of Quantum Information and Quantum Physics
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Santa Cruz, CA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Grant/Contract Number:
AC02-05CH11231; NSC 102-2112-M032-007-MY3; NSC 102-2632-M032-001-MY3; DMR-1420073
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
OSTI Identifier:
1408489